Tatyana Tolstaya, one of his schoolmates, introduced him to her famous father. Sulerzhitsky grew fascinated with Leo Tolstoy's ideas of pacifism and anarchism and decided to dedicate his life to their dissemination. He became one of the most loyal Tolstoyans. His diary kept track of early Doukhobor life before, during, and just after the Doukhobor's migration to Canada at the beginning of the twentieth century. The published diary is called To America with the Doukhobors.

Sulerzhitsky contributed greatly to the construction of one of the most successful actor training techniques in the world. He worked with Constantin Stanislavski for many years. In his book on Stanislavski's 'system' Mel Gordon attributes its founding to Stanislavski's nine-year relationship with Suler. He was well versed in Eastern-influenced religious practices, informing Stanislavski about yoga, meditation and the nature of Prana.